Enhanced stabilization and effective utilization of atomic hydrogen on Pd-in nanoparticles in a flow-through electrode
Enhanced stabilization and effective utilization of atomic hydrogen on Pd-in nanoparticles in a flow-through electrode
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流通电极中 Pd-In 纳米颗粒上原子氢的增强稳定性和有效利用
DOI：
10.1021/acs.est.9b03111
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发表时间：
2019
影响因子：
11.4
通讯作者：
Jiuhui Qu
中科院分区：
文献类型：
--
作者：
Yujun Zhou;Gong Zhang;Qinghua Ji;Wei Zhang;Junyu Zhang;Huijuan Liu;Jiuhui Qu
表面吸附活性物种是多相催化反应中具有较强活性的中间体。这些中间体的有效稳定是提高催化性能的关键。在这里，我们展示了高活性的钯-铟（Pd-In）纳米颗粒（NPs），可以稳定表面上的原子H*，并对溴酸盐显示出有效的电催化还原性能。研究了Pd与In的最佳原子比，目的是有效地形成和强稳定H*，从而促进致癌物溴酸盐的还原和去污。Pd 2 In 3是活性最高的催化剂，具有0.029 min-1的高速率常数，而单金属Pd NPs的速率常数仅为0.009 min-1。密度泛函理论计算表明，Pd 2 In 3 NPs降低功函数，并提供强大的H* 稳定能力。通过采用涂覆有Pd 2 In 3 NPs的流通电极来增强传质，可以提高H* 的利用率，并且还原动力学增加高达7.5倍。
Surface-adsorbed active species are intermediates with strong activities in heterogeneous catalytic reactions. Effective stabilization of these intermediates is crucial to improve the catalytic performance. Here, we demonstrated highly active bimetallic palladium–indium (Pd–In) nanoparticles (NPs) that can stabilize atomic H* on the surface and show efficient electrocatalytic reduction performance toward bromate. The optimal atomic ratio of Pd to In was investigated with the aim of efficient formation and strong stabilization of H*, thus facilitating the reduction and decontamination of carcinogenic bromate. Pd2In3was the most active catalyst, with a high rate constant of 0.029 min–1, whereas the rate constant for monometallic Pd NPs was only 0.009 min–1. Density functional theory calculations suggest that Pd2In3NPs decrease the work function and provide strong H* stabilization ability. By employing a flow-through electrode coated with Pd2In3NPs to enhance the mass transport, the utilization of H* could be boosted and the reduction kinetics increased up to 7.5 times.